基于铁配体物的强化类Fenton体系降解有机污染物

发布时间：2018-07-22 16:09

【摘要】：针对Fenton体系应用于有机污染物降解时亚铁过量投加带来的出水铁污染,以及H2O2费用昂贵等存在的问题,本研究提出了三种基于铁-有机酸配合物的新型Fenton-like体系,并分别辅以电化学、紫外光和超声等三种强化手段(Electro-Fe2+/EDTA、UV/Fe3O4/Ox和US/Fe/TPP),研究它们对活性染料罗丹明B和诺氟沙星等典型难降解有机污染物的快速降解规律,具体内容有:(1)研究了基于均相Fe2+-EDTA的电化学辅助类Fenton体系降解活性染料罗丹明B,Fe2+对罗丹明B的降解效率在3h内达到94.5%,并引入BBD软件进行实验的模拟和优化,实验了不同参数条件对罗丹明B降解效果的影响,研究表明:BBD软件其预测值和试验所得到的实际值很接近,BBD模拟软件对本体系降解罗丹明B具有较高的可靠性,Fe2+:EDTA的比例、p H、罗丹明B浓度以及电压均对罗丹明B的降解效率有影响。(2)研究了Fe3O4-草酸体系对NOR的降解规律,引入UV的协同,实验不同参数条件对NOR的降解效率影响,得出降解NOR的最佳实验参数条件是p H=3、NOR初始浓度为10mg/L、初始Fe3O4浓度为0.5g/L、草酸浓度为1m M,并对不同体系对NOR降解进行了动力学分析,表明UV对体系具有很好的协同作用,探究了降解NOR过程中铁的变化规律,对NOR可能的降解中间产物进行HPLC-MS跟踪,对体系可能对NOR降解起作用的自由基进行捕获剂实验,验证了体系中降解NOR是羟基自由基和超氧自由基以及过氧化氢自由基等共同作用的结果。(3)探究了US-ZVI-TPP体系对NOR的降解,采用EDTA、EDDS、DTPA络合剂与TPP做对比,得出选用TPP络合剂对本体系有很好的降解作用,实验了不同参数对NOR降解效率的影响,得出降解NOR最佳的实验参数条件是p H=7、初始NOR浓度为10mg/L、Fe浓度为1.0g/L、TPP浓度为0.3m M,实验了降解过程中的捕获剂对体系的抑制情况,对NOR降解过程中铁的变化规律进行了研究,并对各参数条件进行了动力学模拟,证明了实验结果的可靠性,研究了降解过程中铁的变化规律,并对各体系降解NOR进行了动力学分析,得出US对体系具有很好的协同作用。
[Abstract]:In order to solve the problems of iron pollution in effluent caused by Fe _ 2O _ 2 overdose and the high cost of H _ 2O _ 2 when Fenton system is applied to organic pollutant degradation, three novel Fenton-like systems based on iron-organic acid complexes are proposed in this paper. The electrochemical, ultraviolet and ultrasonic intensifiers (Electro-Fe _ 2 / EDTA, UV / Fe _ 3O _ 4 / O _ x and US/ Fe / TPP) were used to study the rapid degradation of typical refractory organic pollutants such as Rhodamine B and norfloxacin. The main contents are as follows: (1) the degradation efficiency of Rhodamine B by electrochemically assisted Fenton-like Fenton system based on homogeneous Fe _ 2-EDTA has been studied. The degradation efficiency of Rhodamine B is 94.5g in 3 hours. BBD software is introduced to simulate and optimize the experiment. The effects of different parameters on the degradation of Rhodamine B were studied. The results show that the predicted value and the actual value obtained by the experiment are very close to that of the BBD software. The ratio of Fe2: EDTA, the concentration of Rhodamine B and the voltage of Rhodamine B are all higher than those of Rhodamine B in this system. The results show that the ratio of Fe2: EDTA, the concentration of Rhodamine B and the voltage of Rhodamine B in this system are very high. (2) the degradation of nor in Fe3O4-oxalic acid system was studied. The effect of different parameters on the degradation efficiency of nor was studied by UV synergism. The optimum experimental parameters for the degradation of nor were obtained as follows: the initial concentration of pH3NOR was 10mg / L, the initial concentration of Fe3O4 was 0.5g / L, the concentration of oxalic acid was 1m M.The kinetic analysis of the degradation of nor by different systems showed that UV had a good synergistic effect on the system. The changes of iron in the degradation of nor were studied. The possible degradation intermediates of nor were tracked by HPLC-MS, and the free radicals which might be degraded by the system were tested as trapping agents. It was verified that the degradation of nor in the system was the result of the interaction of hydroxyl radical, superoxide radical and hydrogen peroxide radical. (3) the degradation of nor in US-ZVI-TPP system was investigated, and the EDTA-EDDS- DTPA complex was compared with TPP. It is concluded that the TPP complex agent has a good degradation effect on the system, and the effect of different parameters on the degradation efficiency of nor is tested. The optimum experimental parameters for the degradation of nor were obtained as follows: the initial nor concentration was 10 mg / L ~ (-1) TPP = 0.3 m ~ (-3). The inhibition of the trapping agent on the system was studied, and the variation of iron in the degradation process of nor was studied. The experimental results are proved to be reliable, and the variation of iron in the degradation process is studied. The kinetic analysis of the degradation of nor shows that US has a good synergistic effect on the system.
【学位授予单位】：华中科技大学
【学位级别】：硕士
【学位授予年份】：2015
【分类号】：X703

【相似文献】